Crowd favourite Jabeur carried the hopes of Tunisia, Africa and the Arab world into the showpiece match, but her game fell apart horribly on Centre Court.
"It will be tough to speak because this is very tough," the sixth seed, her eyes wet with tears, said on court after losing in the Wimbledon final for the second year in a row.
"I am going to look ugly in the photos so that's not going to help. I think this is the most painful loss of my career."
Jabeur was also the favourite last year but lost the final to big-hitting Elena Rybakina. When she avenged that loss in this week's quarter-finals and then knocked out second seed Aryna Sabalenka in the semi-finals, it appeared the stars were aligning for her.
All the pre-match talk was of Jabeur being set to become the first African woman and first Arabic player to win a Grand Slam title, having also been runner-up at the 2022 US Open.
But despite winning the first two games, she produced a nervous, mistake-strewn display that was painful to watch at times as her dream faded.
"I want to say congratulations to Marketa and her team for this amazing tournament. You're an amazing player," said Jabeur, who looked devastated at the end of the match.
"It's going to be a tough day for me today. I'm not going to give up. I'm going to come back stronger and win a Grand Slam one day. It was an amazing tournament for me.
"I wished I continued to the end. I want to thank my team for always believing in me. We are going to make it one day, I promise you."
Jabeur, whose inventive playing style and bubbly personality have endeared her to fans around the world, was given a rousing ovation as she walked off to leave the stage for Vondrousova.
"I appreciate your support. It's been a tough journey but that's tennis. I promise I will come back one day and win this tournament," she told the crowd.
